C60 fullerene peapods and double-walled carbon nanotubes (DWCNTs) containing highly 13C enriched C60 and inner tubes, respectively, are studied using Raman spectroscopy and in situ Raman spectroelectrochemistry in order to follow the influence of 13C enrichment on the vibrational pattern of these carbon nanostructures. The Raman response of 13C60 after encapsulation in fullerene peapods differs from that of isotope-natural species, (Nat)C60. The Raman A(g)(2) mode of encapsulated 13C60 is upshifted in frequency compared to that of the (Nat)C60 peapods with the same filling factor. The chemical doping of 13C60 peapods (peapod = C(60)@SWCNT) with K-vapor leads to the downshift of the A(g)(2) mode, similar to the case of (Nat)C60 peapods. The 13C60 peapods were successfully transformed into DWCNTs, which confirms high filling of single-walled (SW) CNTs with 13C60. The DWCNTs exhibited distinctly downshifted G and D Raman modes for inner tubes, which proves that only inner tubes were enriched by 13C. The in situ Raman spectroelectrochemistry of (Nat)C60 exhibits strong anodic enhancement, while for 13C60 peapods the enhancement is only weak. On the other hand, the electrochemical charging of the inner-tube-labeled DWCNTs (13C(i)-DWCNTs) followed the behavior of ordinary (Nat)C(i)-DWCNTs as indicated by in situ Raman spectroelectrochemistry. In addition, the spectroelectrochemical behavior of the G mode of inner tubes in 13C(i)-DWCNTs is followed from the start of the electrochemical doping, which was not feasible for (Nat)C(i)-DWCNTs.